ARTICLE IN PRESS

FOOD

HYDROCOLLOIDS
Food Hydrocolloids 21 (2007) 480486
www.elsevier.com/locate/foodhyd

Synergistic rheological behaviour of mixed HM/LM pectin gels

Caroline Lofgren, Anne-Marie Hermansson
SIK, The Swedish Institute for Food and Biotechnology, P.O. Box 5401, SE-402 29 Goteborg, Sweden
Received 23 September 2005; accepted 6 July 2006

Abstract
The objective of this study was to investigate the rheological behaviour of mixed gels of high methoxyl (HM) and low methoxyl (LM)
pectins with the purpose of designing gels with reduced sucrose content but unaltered rheological properties. The gelation behaviour of
mixed HM/LM pectin gels was compared to that of HM and LM pectin gels in the presence of 30%, 45% and 60% sucrose. The gels
were investigated in the presence of 0.1% CaCl2
2H2O and pH 3.5, conditions that favour the gel formation of both HM and LM
pectins. Strong synergistic effects occurred in the rheological behaviour for three mixed 0.8% HM/0.4% LM pectin gels under conditions
where LM pectin formed microgels instead of coherent gels. The addition of LM pectin strongly increased the storage modulus in mixed
HM/LM pectin gels based on 60% and 45% sucrose compared to HM pectin gels of the same sucrose concentration. The kinetic
behaviour of the mixed HM/LM pectin gels during gel formation varied depending on the kinetic behaviour of the HM pectins differing
in degrees of blockiness. Transmission electron microscopy (TEM) showed that the gel microstructure of the mixed gel with 60% sucrose
was inhomogeneous. The addition of HM pectin in mixed gels with only 30% sucrose increased the storage modulus two to ve times
compared to that of 0.4% LM pectin gels under the same conditions. The phase angle for the mixed gel with 30% sucrose was also higher
than for the corresponding 0.4% LM pectin gel.
r 2006 Elsevier Ltd. All rights reserved.
Keywords: HM pectin; LM pectin; Mixed gels; Gel formation; Rheology; Sucrose

1. Introduction
The increasing demand for food products with reduced
sugar content challenges the food industry to develop
healthy products without affecting texture and sensory
properties. Pectins with their gelling and stabilising properties constitute interesting candidates in the development of
low sugar applications. The major component of pectin is
a-(1-4)-D-galacturonic acid (GalA) units in which some of
the carboxyl groups can be substituted with methyl esters
or amide groups (Voragen, Pilnik, Thibault, Axelos, &
Renard, 1995). High methoxyl (HM) pectins, with more
than 50% of the carboxyl groups esteried, form gels
mainly by hydrophobic interactions and hydrogen bonds at
pHp3.5 and in the presence of more than 55% sugar
(Oakenfull & Scott, 1984). Low methoxyl (LM) pectins,
with less than 50% of the carboxyl groups esteried, are
often used in low-sugar products due to their gel-forming
Corresponding author. Tel.: +46 31 335 56 58; fax: +46 31 83 37 82.

E-mail address: amh@sik.se (A.-H. Hermansson).

0268-005X/$ - see front matter r 2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.foodhyd.2006.07.005

properties without or with a small amount of sugar and in

the presence of Ca2+. At high sucrose concentrations LM
pectin tends to pregel (May, 1990). Gel formation of LM
pectin occurs over a wide range of pH values, and the
efcient Ca2+-binding is an important factor both at low
and high pH values (Cardoso, Coimbra, & Lopes da Silva,
2003). The distribution of free and esteried carboxyl
groups in the pectin backbone affects the strength of the
Ca2+-binding and thus the functionality of both LM and
HM pectin gels (Lofgren, Guillotin, Evenbratt, Schols, &
Hermansson, 2005; Powell, Morris, Gidley, & Rees, 1982).
Mixtures of pectins are often used in food applications to
obtain products with certain functionalities. It was shown
previously that large variations in rheological behaviour
and microstructure can be obtained in mixtures of HM and
LM pectin gels by altering the gel formation conditions
(Lofgren, Walkenstrom, & Hermansson, 2002). A strong
synergistic effect in the rheological properties was obtained
for a mixed HM/LM pectin gel in the presence of Ca2+ and
60% sucrose at pH 3, i.e. under conditions that facilitate
the gel formation of both HM and LM pectin. The kinetic

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C. Lofgren, A.-H. Hermansson / Food Hydrocolloids 21 (2007) 480486

behaviour of a mixed HM/LM pectin gel in the absence of

calcium showed characteristics of both HM and LM pectin
gelation at pH 3 (Lofgren & Hermansson, 2004). The HM
pectin sample showed a rather slow gel formation in the
presence of 60% sucrose. The LM pectin also formed a gel,
despite the absence of calcium. A weak gel was rapidly
formed due to the acidic conditions and the presence of
60% sucrose. Consequently, the mixed HM/LM pectin gel
showed a rapid initial increase followed by a progressive
increase during the latter part of the measurement.
Results from transmission electron microscopy revealed
that the microstructure of HM, LM and mixed pectin gels
differed greatly. Gels of HM and LM pectin at pH 3 were
composed of open networks with pores in the range of
500 nm. A mixed HM/LM pectin gel with 60% sucrose in
the absence of calcium had a ne-stranded gel structure
with much smaller pores, whereas in the presence of both
calcium and 60% sucrose a highly inhomogeneous gel
structure was obtained.
The kinetic behaviour during gelation of pectins is an
important factor in the manufacture of many food
products. In jams with large fruit pieces, for example, it
is useful to have a fairly rapid-set pectin to ensure that the
fruit is evenly distributed. In other cases where the most
important issue is to obtain a clear gel product without air
bubbles, a slow set pectin is preferred (May, 1992). An
increased degree of esterication (DE) results in a more
rapid gel formation of HM pectins, and it has also been
shown that the distribution of methyl esters affects the
kinetic behaviour of HM pectin gels. For three comparable
pectins having DE 75%, the shortest gelation time was
obtained for the most blockwise-distributed sample.
Furthermore, the addition of Ca2+ resulted in faster gel
formation for the HM pectins (Lofgren et al., 2005). The
concentration of Ca2+ is also crucial for the kinetic
behaviour of LM pectin gels. It has been demonstrated
for LM pectin gels at pH 6 that increased Ca2+
concentration results in faster gel formation (Lootens
et al., 2003).
The objective of this study was to gain information on
the functionality of HM and LM pectin mixtures so that
mixed gels with reduced sucrose content but the same
rheological properties as HM pectin gels of higher sucrose
concentrations can be designed. We have investigated the
gel formation behaviour and rheological properties of
mixed HM/LM pectin gels at 30%, 45% and 60% sucrose.
Three different HM/LM pectin mixtures have been studied
in the presence of calcium at pH 3.5, conditions that
facilitate the gel formation of both HM and LM pectins.
2. Materials and methods
2.1. Materials
The pectin samples A, B and C30 were kindly provided
by the Laboratory of Food Chemistry, Wageningen
University (Wageningen, the Netherlands). The HM

481

pectins A and B originate from the same lemon variety

and have comparable degrees of esterication (DE of 74%
and 72%, respectively) but differ in the distribution of
methyl esters. The degree of blockiness (DB) was 16% for
pectin A and 5% for pectin B. A high DB value indicates
the release of a high number of mono-, di- and tri-GalA
and consequently a blockwise distribution of nonesteried
galacturonic acid residues in a pectin (Guillotin et al.,
2005). The molecular weight (Mw), determined with highperformance size exclusion chromatography (HPSEC), was
 82 kDa for pectin A and 78 kDa for pectin B. The LM
pectin C30 had a DE of 30% and DB of 16.5%. The pectin
samples HMC and LMC, kindly provided by Danisco A/S,
(Denmark) were unstandardized (without added sugar).
The Ca2+-sensitive HMC pectin had a DE of 70% and the
LMC pectin had a DE of 33%. The Ca2+sensitivity was
related to a viscosity increase in the pectin in solution when
calcium was added compared to the same solution without
calcium.
A constant CaCl2
2H2O-concentration of 0.1% was
used throughout the study. A recent work by Guillotin
(2005) shows that commercial pectins in general are
mixtures of several subpopulations. The DE values vary
among these populations and it is therefore not adequate to
relate the Ca2+-concentration to the DE value or COOHconcentration.
2.2. Sample preparation
The pectins were dissolved in 0.1 M citrate buffer at pH
3.5 and stirred at room temperature for 90 min. The
samples were heated to 95 1C in an oil bath with a
temperature of 110 1C. A preheated solution of 1.8 ml
CaCl2 in citrate buffer was added to the samples dropwise
under continuous stirring, giving a nal concentration of
0.1% CaCl2
2H2O in the samples. The samples were reheated to 95 1C and sucrose was added. For the samples
containing 1.2% pectin and 60% sucrose, the procedure
was slightly different. Sucrose was added before the
addition of the Ca2+-solution to ensure that the sugar
was completely dissolved in the sample. The weight of each
sample was adjusted with distilled water, and the samples
were re-heated to 95 1C before they were poured into the
rheometer cup. To prepare them for microscopy, the
samples were poured into glass beakers and stored at room
temperature.
2.3. Rheological measurements
The rheological properties during gel formation were
characterized by oscillatory measurements in a Stresstech
rheometer (Reologica Instruments, Lund, Sweden) with
strain-controlled oscillation in a cup and bob geometry at
20 1C. The surface of the sample was covered with parafn
oil to avoid evaporation. The temperature of 20 1C was
obtained 8 min after the measurement started. Gel
formation measurements were performed at a frequency

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C. Lofgren, A.-H. Hermansson / Food Hydrocolloids 21 (2007) 480486

482

of 1 Hz and a strain of 2  103 for 3 and 16 h. Frequency

sweeps were performed on the gels 16 h after gel formation.

compared to HM and LM pectin gels with a concentration

of 1.2% and also to 0.8% HM pectin gels and 0.4% LM
pectin gels.

2.4. Microscopy
3.1. An increased storage modulus in pectin mixtures
Small gel cubes 1  1  1 mm were cut from the bulk
gels 20 h after gel preparation. The gels were xed in an
aldehyde solution, based on citrate buffer, 2% glutaraldehyde and 0.1% ruthenium red. The citrate buffer contained
50% sucrose and 0.1% CaCl2
2H2O. The gel cubes were
placed in the xation solution for 20 h. The microscopy
samples were then dehydrated, polymerized and thinsectioned according to a previous method (Lofgren et al.,
2002). The samples were examined with a transmission
electron microscope (LEO 906E Electron Microscopy Ltd.,
Cambridge, England) at 80 kV.

In Fig. 1 the three mixed pectin gels are compared to

HM pectin gels with a total pectin concentration of 1.2%
at 60% sucrose (Figs. 1ac) and 45% sucrose (Figs. 1df).
All mixtures exhibit a signicantly higher storage modulus
than the corresponding HM pectin gels of 1.2%. The
corresponding LM pectin samples of 1.2% do not form
coherent gels but rather thick grainy pastes, i.e. microgels,
in all cases except for the LMC gel in the presence of 45%
sucrose.
The HM/LM pectin mixtures results in G0 values many
times higher than those of the HM pectin gels at the same
sucrose concentration, and it is interesting that mixed HM/
LM gels at 45% sucrose show G0 values of the same
magnitude as for HM gels with 60% sucrose, e.g. pectin A
in Fig. 1a can be compared with A-C30 in Fig. 1d. For the
mixed B-C30 gel with 45% sucrose an even higher G0 is
obtained than for pectin B with 60% sucrose (Figs. 1b and
e). The gel-formation ability of pectin A in the presence of
only 45% sucrose is probably a result of the high
blockiness in the sample, which facilitates Ca2+ bindings
to blocks of non-esteried GalA units. No gel formation
occurred for pectin B and HMC in the presence of 45%
sucrose, as indicated by dotted lines in Figs. 1e and f.

3. Results and discussion

The gel formation behaviour was investigated for HM,
LM and mixed pectin gels in the presence of 0.1%
CaCl2
2H2O at pH 3.5 at three different sucrose concentrations: 30%, 45% and 60%. Three HM/LM pectin
mixtures were investigated: A-C30, composed of the
blockwise HM pectin A and the LM pectin C30, B-C30,
composed of the random HM pectin B and the LM pectin
C30, and HMC-LMC, composed of the Ca2+-sensitive
HM pectin HMC and the LM pectin LMC. The mixed
gels, based on 0.4% LM pectin and 0.8% HM pectin, were
800

60% sucrose G' (Pa)

3500
3000

HMC-LMC

2000

600

A-C30
400

400

1500
1000

200

500

B
0

(a)

HMC

200

A
0

12

16

0
0

(b)

time (h)

12

16

(c)

time (h)

time (h)

250

250

350

45% sucrose G' (Pa)

B-C30

600

2500

B-C30

300

A-C30

200

200

150

150

100

100

50

50

250
200
150

HMC-LMC

100

50
0

8
time (h)

12

16

(e)

HMC

(d)

800

0
8
time (h)

12

16

(f)

2
time (h)

Fig. 1. The storage modulus during gel formation in mixed 0.8% HM/0.4% LM pectin gels compared to 1.2% HM pectin gels: (a) A-C30 and A with 60%
sucrose; (b) B-C30 and B, 60% sucrose; (c) HMC-LMC and HMC, 60% sucrose; (d) A-C30 and A, 45% sucrose; (e) B-C30 and B, 45% sucrose; and (f)
HMC-LMC and HMC, 45% sucrose.

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C. Lofgren, A.-H. Hermansson / Food Hydrocolloids 21 (2007) 480486

10000
A, A-C30

1000
G' G'' (Pa)

All mixtures show a rapid gel formation with G0 4G00

from the beginning of the measurement, but the development in G0 during the measurement period differs. The
mixture of the blockwise pectin A and C30 with 60%
sucrose shows a strong, progressive increase in G0 over a
period of 16 h (Fig. 1a). The storage modulus increases by
more than 300% from 0.5 to 16 h. In comparison, the
storage modulus of pectin A increases by 150% from 0.5
to 16 h. Another kinetic behaviour is observed for the
mixed gel of B and C30 and the gel of pectin B. After a
rapid initial increase, G0 increases by only 60% for the
mixed gel and by 30% for the gel of pectin B from 0.5 to
16 h. A progressive increase in G0 can also be seen for HMC
and mixed HMCLMC gels at 60% sucrose (Fig. 1c).
The magnitude of the storage modulus in the mixed gels
is strongly affected by the reduction of sucrose from 60%
to 45%. The efciency of the HM pectins is reduced by the
low sucrose concentration. However, similar kinetic
behaviour occurs for HM and mixed gels at both 60%
and 45% sucrose, but in the presence of 45% sucrose the
increase in G0 is generally smaller than at 60% sucrose (G0
increases with 90% for the mixed A-C30 gel and with
30% for the mixed B-C30 gel from 0.5 to 16 h). In an
earlier investigation, it was shown that the shape of the G0
curve was the same for LM pectins both without and with
30% sucrose. The gels thus showed similar kinetic
behaviour during gel formation both with and without
sucrose although the presence of sucrose strongly increased
the storage modulus of the gels (Lofgren, Guillotin, &
Hermansson, 2006). The present results demonstrate that
the kinetic behaviour of the HM pectins has a strong
bearing on the kinetic properties of the mixed gels.
Not only the storage modulus but also the phase angle d
is affected when the composition of the gels is changed
from HM pectin to mixed HM/LM pectins. The presence
of LM pectin results in gels with a lower phase angle, i.e.
the viscous part of the gels is lower than in the
corresponding HM pectin gels both at 60% and 45%
sucrose (see Table 1). The high phase angle observed for
HM pectin gels is a result of the high pH value (3.5), which
is close to the upper limit for HM pectin gelation. Gel
formation of HM pectins only occurs when the pH value is
sufciently low to suppress the electrostatic repulsions
between charged carboxyl groups, thus facilitating hydro-

gen bonds and hydrophobic interactions between the

pectin molecules. The mechanical spectra of HM pectin
gels and mixed HM/LM pectin gels recorded 16 h after the
gel formation are shown in Fig. 2. The frequency response
of A and A-C30 in Fig. 2a shows a typical gel-like
behaviour with G0 bG00 (Clark & Ross-Murphy, 1987) and
also a slight increase in G0 when the frequency increases.
Pectins B and B-C30 (Fig. 2b) show a somewhat higher
frequency dependence than A and A-C30 and, due to the
high phase angle of gels based on pectin B, there are also
smaller differences in magnitude between G0 and G00 . This
behaviour is often observed for weak cross-linked network
structures (Evageliou, Richardson, & Morris, 2000; Tsoga,
Richardson, & Morris, 2004). The results show that the
substitution of HM pectin to a mixture of HM/LM pectin
leads to considerably higher dynamic moduli without any
larger effects on the frequency behaviour.

100

10
0.01

0.1

10

10

frequency (Hz)

(a)
10000
B, B-C30

1000
G' G'' (Pa)

3.2. Rheological behaviour of mixed gels in relation to HM

pectin gels

483

100

Table 1
Phase angle after 16 h (d16) for 1.2% HM pectin and mixed (0.8%HM/
0.4%LM) pectin gels with 60% and 45% sucrose
HM pectin gels

d16 h

HM/LM pectin gels

d16 h

A, 60% s.
B, 60% s.
A, 45% s.
B, 45% s.

10
33
31
68

A-C30, 60% s.
B-C30, 60% s.
A-C30, 45% s.
B-C30, 45% s.

7
16
12
14

10
0.01
(b)

0.1
frequency (Hz)

Fig. 2. Frequency sweeps of 1.2% HM pectin gels (solid lines) and mixed
0.8% HM/0.4% LM pectin gels (dotted lines) in the presence of 60%
sucrose 16 h after gel formation. G0 black, G00 grey.

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C. Lofgren, A.-H. Hermansson / Food Hydrocolloids 21 (2007) 480486

484

HM and LM pectin gels

Mixed HM/LM pectin gels

1500

40

1.2% A-C30
0.8% A

1000

30

G' (Pa)

60% sucrose G' (Pa)

50

0.8% B

20
10
0

0
0

time (h)

(a)

time (h)

(b)

30

30

20

20

1. 2%

G' (Pa)

30% sucrose G' (Pa)

1.2% B-C30

500

1. 2%

A -C 3 0

B -C 3 0

10

10
0.4% C30

0
0

(c)

time (h)

(d)

time (h)

Fig. 3. Mixed 0.8% HM/0.4% LM pectin gels compared to HM pectin gels of 60% and LM pectin gels of 30% sucrose. The dotted line indicates that no
gel formation occurred in the sample.

3.3. The influence of the non-favoured pectin in mixed gels

The gel-formation ability of HM and LM pectins is
generally limited to different sugar concentrations. HM
pectins normally form gels when water activity is reduced,
i.e. in the presence of 55% cosolute or more. The reduced
water activity facilitates hydrophobic interactions between
the methyl esters. LM pectin gelation is favoured at low
sugar concentrations and tends to form microgels at high
sucrose concentrations in the presence of Ca2+. However,
the presence of the non-favoured pectin can affect the
rheological properties in pectin mixtures. In Fig. 3 the
mixed A-C30 and B-C30 gels are compared to 0.8% HM
pectin gels of A and B and to 0.4% C30 in the presence of
60 and 30% sucrose.
3.3.1. The influence of LM pectin on HM pectin gelation
The HM pectins A and B form rather weak gels in the
presence of 60% sucrose, whereas the LM pectin C30
forms microgels under the same conditions. The strong
aggregation of C30 in the presence of 60% sucrose gives
rise to a strong contribution to the mixed gels, as can be
seen in Fig. 3b. It is interesting that the addition of 0.4%
LM pectin can result in a more than 30 times higher
storage modulus after 3 h (G0 3 h) in the mixed gel with 60%
sucrose compared to that in 0.8% HM pectin gel. In a

mixture of both HM and LM pectins, it is likely that the

strong LM pectinCa2+ interaction resulting in microgels
is diminished due to the presence of HM pectin. However,
LM pectinCa2+ clusters may occur in a mixed gel
surrounded by a coherent gel network of HM pectin, as
indicated in the inhomogeneous microstructure of A-C30
in Fig. 4. In contrast, pectin A forms a homogeneous gel
structure at pH 3.5 with 60% sucrose and calcium (results
not shown). In comparison, a highly inhomogeneous mixed
HM/LM (50/50) gel composed of dense LM pectin-rich
areas and sparse HM pectin-rich areas was formed in the
presence of 60% sucrose and calcium at pH 3 (Lofgren
et al., 2002). In that case, more distinct dense areas were
obtained compared to the density uctuations seen in
Fig. 4. An explanation could be that LM pectin forms
stronger aggregates at pH 3 than at pH 3.5 in the presence
of Ca2+ due to the suppressed electrostatic repulsions
occurring at low pH values. Furthermore, a more rapid gel
formation of HM pectin occurs at pH 3 than at pH 3.5,
possibly contributing to a more inhomogeneous gel
structure at pH 3.0 than at pH 3.5.
3.3.2. The influence of HM pectin on LM pectin gelation
The effect of HM pectin in the mixed gel with 30%
sucrose is less dramatic than the effect of LM pectin in
mixed gels with 60% sucrose. No gel formation occurs for

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C. Lofgren, A.-H. Hermansson / Food Hydrocolloids 21 (2007) 480486

the HM pectin B with 30% sucrose and Ca2+, whereas a

weak gel is slowly formed for pectin A under the same
conditions due to the blockwise distribution of methyl
esters (see Fig. 5). The presence of pectins A and B affects

Fig. 4. Gel microstructure of a mixed 0.8% HM/0.4% LM (A-C30) pectin

gel with 60% sucrose.

G' G'' (Pa)

15

10

485

the storage modulus in the mixed gels (Figs. 3c and d). The
mixed A-C30 gel shows about a ve times higher G0 3 h
compared to the LM pectin gel, and the mixed B-C30
shows about a two times higher G0 3 h compared to the LM
pectin gel. It is likely that both pectins A and B support the
gel structure formed by the LM pectin to some extent.
Furthermore, the presence of HM pectins results in gels of
higher viscous properties in the presence of 30% sucrose.
The phase angle after 3 h is 15 for the 0.4% LM pectin and
20 for the mixed HM/LM pectin gels. The enhanced
phase angle indicates that the HM pectins increase the
polymer concentration in the watersucrose phase and
thereby the viscous properties of the gels. In a previous
work, a mixture of equal amounts of HM and LM pectins
(0.75%/0.75%) based on 30% sucrose and Ca2+ was
compared to a 0.75% LM pectin gel under the same
conditions. In similarity with the present result, the viscous
properties (as indicated by G00 ) were higher in the mixed gel
than in the LM pectin gel. However, no signicant increase
in G0 was detected for the mixed gel composed of equal
amounts of HM and LM pectins compared to the LM
pectin gel (Lofgren et al., 2002).
Interestingly, a similar relation to that between mixed
gels of 45% sucrose and HM pectin gels of 60% sucrose
(Fig. 1) was found at lower sucrose concentrations. The
mixed A-C30 gel with 30% sucrose (Fig. 3d) shows a G0 of
the same magnitude as that for the gel of 1.2% pectin A
with 45% sucrose (Fig. 1d).
3.4. Effect of sucrose

0
0

12

time (h)
Fig. 5. Gel formation of 1.2% pectin A in the presence of 30% sucrose.
G0 black line, G00 grey line.

The storage modulus is strongly affected by the sucrose

concentration, as can be seen for a mixture of 1.2% A-C30
in Fig. 6a. When the sucrose concentration increases, the
water activity is reduced. The increase in the effective
pectin concentration that occurs may also contribute
to the increased storage modulus in the samples. The
pectin concentration was adjusted so that the same ratio of
pectin to solution (citrate buffer) was obtained at all
sucrose concentrations. The variations in effective pectin

1500
A. 1.2% pectin, 60% sucrose (0.031)
B. 1.2% pectin, 45% sucrose (0.022)
C. 1.2% pectin, 30%sucrose (0.017)

D. 0.87% pectin, 60% sucrose (0.022)

E. 1.2% pectin, 45% sucrose (0.022)
F. 1.5%pectin, 30% sucrose (0.022)

G' (Pa)

1000
A
500
D
B

0
0

(a)

C
2

1
time (h)

(b)

time (h)

Fig. 6. The effect of sucrose in G0 for A-C30 mixtures (2/3 A and 1/3 C30) during gel formation. The numbers within brackets indicate the pectin:solution
ratio of the samples (w/w).

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C. Lofgren, A.-H. Hermansson / Food Hydrocolloids 21 (2007) 480486

concentration were thus excluded. In Fig. 6b three mixtures

differing in sucrose concentration but with the same
pectin:solution ratios are compared. It can be seen that
increased sucrose concentration results in an increased
storage modulus even when the samples have the same
pectin:solution ratio, i.e. the same effective pectin concentration, but the differences are much smaller than for
samples based on 1.2% pectin (Fig. 6a). The results in
Fig. 6 show that both the sucrose concentration and the
effective pectin concentration contribute to the changes in
the storage modulus.
In a previous paper, a strong synergistic effect was
observed in the presence of Ca2+ for a HM/LM pectin
mixture at pH 3 with 60% sucrose (Lofgren et al., 2002).
The present work shows that the synergism is also very
pronounced at pH 3.5, at different sucrose concentrations
and for several pectin mixtures differing in kinetic
behaviour and Ca2+ sensitivity. The results imply that, in
rheological terms, a HM pectin gel of 60% sucrose can be
substituted with a mixed HM/LM pectin gel of 45%
sucrose. In addition, a HM pectin gel of 45% sucrose can
be substituted with a mixed HM/LM pectin gel of 30%
sucrose. The results demonstrate the possibility of using
pectin mixtures with a reduced sucrose content without
altering their rheological and kinetic properties.

4. Conclusions
This study showed that a strong synergistic effect in the
storage modulus occurred in mixed HM/LM pectin gels
compared to HM pectin gels of the same concentration and
under conditions where LM pectin did not form coherent
gels. Mixed HM/LM pectin gels exhibited similar rheological behaviour to HM pectin gels of higher sucrose
concentrations. Different kinetic behaviour during gel
formation was obtained for the mixed gels depending on
the kinetic behaviour of the HM pectins. The addition of
the LM pectin increased the storage modulus about 30
times for mixed gels based on 60% sucrose. The strong
aggregation of LM pectin in the presence of 60% sucrose
and calcium contributed to a large effect on the storage
modulus of the mixed gels. An inhomogeneous gel
structure was revealed, which indicated the presence of
LM pectinCa2+-rich domains in the mixed gel based on
60% sucrose.
The addition of HM pectin in mixed gels based on 30%
sucrose increased the storage modulus two to ve times
compared to that of 0.4% LM pectin gels and under
conditions where HM pectin formed no or very weak gels.
Furthermore, the addition of HM pectin also increased the
phase angle and thus the viscous properties of the mixed
gels at 30% sucrose. This work showed that the magnitude
of the storage modulus was affected by both the sucrose
concentration and the effective pectin concentration of
the gels.

Acknowledgements
The authors would like to thank Preben B. Rasmussen
and Karen Marie Sondergaard at Danisco A/S and Henk
Schols and Stephanie Guillotin at Wageningen University
for kindly providing materials to the study. This project is a
part of the LiFT programme (Future Technologies for
Food Production), nanced by the Swedish Foundation for
Strategic Research (SSF).
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